JP2001235547A - High sensitivity nuclear species analysis method by multiple gamma ray detection - Google Patents
High sensitivity nuclear species analysis method by multiple gamma ray detectionInfo
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Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、多重ガンマ線検出
法を放射性核種又は中性子その他の粒子線或いはガンマ
線により放射化された試料中の核種の定性、定量に利用
したものであって、その核種から放出される多重ガンマ
線を同時測定して、各核種からのガンマ線対（ペア）の
情報を取ることにより、従来のガンマ線測定よりも高分
解能で分析するものである。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to the use of a multiplex gamma ray detection method for the qualitative and quantitative determination of radionuclides or neutrons or other nuclides in a sample activated by particle beams or gamma rays. Simultaneous measurement of emitted multiple gamma rays and obtaining information of gamma ray pairs from each nuclide enable analysis with higher resolution than conventional gamma ray measurement.
【０００２】即ち、本発明は、放射性核種から放出され
る複数の同時発生ガンマ線を複数のガンマ線検出検出器
からなる多重ガンマ線検出装置により同時計数測定して
得られる２次元マトリクスを解析する方法であり、これ
により複数核種の完全分離と同時分析が可能になった。That is, the present invention is a method for analyzing a two-dimensional matrix obtained by simultaneously counting and measuring a plurality of simultaneous gamma rays emitted from radionuclides by a multiplex gamma ray detector comprising a plurality of gamma ray detectors. This enabled complete separation and simultaneous analysis of multiple nuclides.
【０００３】即ち、従来の分析法では約１０００分の１
の分解能が得られるが、本発明の新しい２次元マトリク
スを解析する法では更に１０００分の１である百万分の
１の分解能が達成される。これより、いかに多くの核種
を含む試料であろうとも核種の完全分離が可能になる。
現実にはあり得ないことであるが、これまでに存在が知
られている最大２０００−３０００の核種が、加速器・
原子炉で同時に作られた場合でも、各々が平均１０本程
度のガンマ線を出すので、ガンマ線の総数は最大１万本
のオーダーであるが、２次元マトリクス解析法における
上記百万分の１の分解能では、これらを同時に定量する
ことが可能になる。That is, in the conventional analysis method, about 1 / 1,000
Although the new method of analyzing a two-dimensional matrix of the present invention achieves a resolution of 1/1000 which is one thousandth of that of the present invention. This enables complete separation of nuclides, no matter how many samples contain nuclides.
Although it is impossible in reality, up to 2000-3000 nuclides known to exist are
Even if they are produced simultaneously in a nuclear reactor, each emits about 10 gamma rays on average, so the total number of gamma rays is up to the order of 10,000, but the resolution of 1 / million above in the two-dimensional matrix analysis method Then, these can be simultaneously quantified.
【０００４】[0004]
【従来の技術】従来行われてきた放射能分析は、放射性
核種から発せられるガンマ線を、１台のゲルマニウム半
導体検出器により測定して得られる一次元のエネルギー
スペクトルから、エネルギーや半減期の情報に基づいて
核種の同定を行っている。このゲルマニウム検出器の分
解能は、１ＭｅＶで約１０００分の１である。放射性核
種は平均して１０本オーダーのガンマ線を放出するの
で、少ない核種を含む試料では問題ないが、数十核種を
含む試料ではガンマ線の本数は数百本に達し、これらを
すべて分離することは不可能になる。特に、弱いガンマ
線は他の強いガンマ線に邪魔されて観測することはでき
ない。2. Description of the Related Art Conventionally, radioactivity analysis is performed by converting gamma rays emitted from radionuclides from a one-dimensional energy spectrum obtained by measuring with a single germanium semiconductor detector into information on energy and half-life. The nuclides are identified based on the results. The resolution of this germanium detector is about 1/1000 at 1 MeV. Since radionuclides emit gamma rays on the order of 10 on average, there is no problem in samples containing a small number of nuclides, but in samples containing tens of nuclides, the number of gamma rays reaches several hundred, and it is impossible to separate them all. Becomes impossible. In particular, weak gamma rays cannot be observed because they are obstructed by other strong gamma rays.
【０００５】また、同様にして、放射性でない試料を加
速器や原子炉からの粒子によって放射化し、その試料か
ら発せられるガンマ線を検出し、その強度を測定する事
により試料の定性、定量分析を行う事もできる。そこ
で、中性子放射化分析法は、試料に原子炉からの中性子
を照射して放射化し、これを単一の高分解能ゲルマニウ
ム検出器で測定し、得られた一次元スペクトル中のピー
クを解析し定量を行う方法である。Similarly, a non-radioactive sample is activated by particles from an accelerator or a nuclear reactor, gamma rays emitted from the sample are detected, and the intensity is measured to perform qualitative and quantitative analysis of the sample. Can also. Therefore, the neutron activation analysis method irradiates a sample with neutrons from a nuclear reactor, activates it, measures it with a single high-resolution germanium detector, analyzes the peaks in the obtained one-dimensional spectrum, and quantifies it. How to do.
【０００６】このような分析は従来より様々な方法によ
り多くの分野で行われており、その中でも上記放射能分
析は広く用いられている。特に1960年代にゲルマニウム
半導体検出器が開発されてからは、高い分解能で検出で
きるガンマ線を用いた放射化分析が発達し、環境試料、
生体試料、宇宙地球科学的試料など様々な試料中の微量
元素の含有量測定が可能となった。[0006] Such analysis has been conventionally performed in various fields by various methods, and among them, the above-mentioned radioactivity analysis is widely used. In particular, since the germanium semiconductor detector was developed in the 1960s, activation analysis using gamma rays that can be detected with high resolution has developed, and environmental samples,
It has become possible to measure the content of trace elements in various samples such as biological samples and space earth science samples.
【０００７】しかし、従来の検出法においては、図１に
示されるように、原子炉からの熱中性子照射による放射
化試料１から発生したガンマ線を単一のゲルマニウム検
出器２で測定し、縦軸をカウント（強さ）、横軸をガン
マ線エネルギーとした１次元スペクトル３を作成する。
この方法では、試料が多元素を含む場合には複雑なスペ
クトルになり、求める元素の分離測定は困難な場合があ
った。However, in the conventional detection method, as shown in FIG. 1, gamma rays generated from an activated sample 1 due to thermal neutron irradiation from a nuclear reactor are measured by a single germanium detector 2 and the vertical axis is measured. Is counted (intensity), and a one-dimensional spectrum 3 is created with the horizontal axis representing gamma ray energy.
In this method, when the sample contains multiple elements, the spectrum becomes complicated, and it is sometimes difficult to separate and measure the desired elements.
【０００８】[0008]
【発明が解決しようとする課題】従来の方法では、混在
する他の核種からの妨害を受け易い。運よく他のガンマ
線と重ならながった場合でも、多核種の場合ではスペク
トル中のバックグランドが高くなり、弱いガンマ線を検
出することは困難になる。The conventional method is susceptible to interference from other mixed nuclides. Even if it does not overlap with other gamma rays fortunately, the background in the spectrum is high in the case of multinuclides, making it difficult to detect weak gamma rays.
【０００９】よって、使用済み核燃料等の多くの核種を
含む試料では妨害となる核種の影響を取り除くために、
一般的には化学分離を行う、あるいは核種の半減期によ
って振り分けるなどの方法が取られる。しかしながら、
化学分離には一般的に特殊な技術と手間が必要であるば
かりでなく、化学分離の収率を求める必要があり、この
操作中に誤差が入り込む可能性がある。又、半減期によ
って振り分ける方法とは、例えば半減期の長い核種を定
量するためにかなりの時間を要し、又その間検出器系を
維持する手間も大変である。Therefore, in order to remove the effects of nuclides that interfere with samples containing many nuclides such as spent nuclear fuel,
Generally, a method such as performing chemical separation or sorting by nuclide half-life is used. However,
Chemical separation generally requires not only special techniques and labor, but also the need to determine the yield of the chemical separation, which can introduce errors during this operation. Also, the method of sorting by half-life requires a considerable amount of time to quantify nuclides having a long half-life, for example, and it is also troublesome to maintain the detector system during that time.
【００１０】これら従来の手法では混在する他の核種か
らの妨害を受けやすいので、環境試料のように多くの元
素が混在している試料では妨害となる核種の影響を取除
くために化学分離等を行う必要があり、それに伴い化学
分離の収率を求めるために再放射化などの操作を行わな
ければならないが、化学分離を行う事により多くの技術
と手間が必要であり、またこの操作中に誤差が入り込む
可能性がある。[0010] Since these conventional methods are susceptible to interference from other mixed nuclides, a sample in which many elements are mixed such as an environmental sample is subjected to chemical separation or the like in order to remove the influence of the interfering nuclides. It is necessary to perform operations such as re-activation in order to obtain the yield of chemical separation.However, performing chemical separation requires a lot of techniques and labor, and during this operation May have an error.
【００１１】また、原子炉から中性子を照射し放射化し
た試料を、単一のゲルマニウム検出器で測定して得られ
た一次元スペクトル中のピークを解析し定量してきた
が、多くの元素を含む試料の場合には生成放射能の相対
強度は一部の核種に偏り、微量元素の同定は困難であ
り、化学分離を併用することが多く、分離後の回収率の
誤差などが最終結果に影響を与えるばかりでなく、化学
分析の技術が必要である。Further, a sample obtained by irradiating neutrons from a nuclear reactor and activating the same is analyzed and quantified in a one-dimensional spectrum obtained by measuring with a single germanium detector, but contains many elements. In the case of samples, the relative intensity of generated radioactivity is biased to some nuclides, it is difficult to identify trace elements, and chemical separation is often used, and errors in the recovery rate after separation affect the final result In addition to the above, a technique of chemical analysis is required.
【００１２】更に、上記中性子放射化分析法でも、一般
的に生成放射能の相対強度は一部の核種に偏り、多くの
微量元素を同時に分析することは困難であることが多
い。例えば生体試料では24Na、56Mn、42K、82Br、また
地質学的試料では 24Na、56Mn、42K、46Sc、59Feのなど
の放射能が強いため、単一の検出器による一次元スペク
トルを解析する方法では、他の短寿命核種のピークがこ
れらに隠れて検出されない。そのため、化学分離により
強い放射核種を除いた後に放射線測定を行うなどの必要
がある。しかしこのためには化学分析の技術が必要なだ
けでなく、化学分離を行った後に原子炉において再放射
化を行い、目的核種の回収率を求めなくてはならない。
さらに化学分離の操作を経る事により分析の精度に影響
を与える事も懸念される。Furthermore, even in the above-mentioned neutron activation analysis method, the relative intensity of generated radioactivity is generally biased to some nuclides, and it is often difficult to analyze many trace elements at the same time. For example, biological samples have high radioactivity such as 24 Na, 56 Mn, 42 K, and 82 Br, and geological samples have high radioactivity such as 24 Na, 56 Mn, 42 K, 46 Sc, and 59 Fe. In the method of analyzing a one-dimensional spectrum according to the above, peaks of other short-lived nuclides are hidden by these and are not detected. Therefore, it is necessary to perform radiation measurement after removing strong radionuclides by chemical separation. However, this requires not only the technique of chemical analysis, but also the re-activation in the reactor after chemical separation, and the recovery rate of the target nuclide must be obtained.
Furthermore, there is a concern that the accuracy of the analysis may be affected by the operation of chemical separation.
【００１３】[0013]
【課題を解決するための手段】本発明は、多くの放射性
核種が複数のガンマ線を放出している事に着目して、こ
れらを複数のガンマ線検出器からなる多重ガンマ線検出
装置により測定して得られる２次元マトリクスを解析す
ることにより、これらの核種を定性、定量する方法を考
案した。この方法により、従来の１次元のスペクトルに
比べ１０００倍のエネルギー分解能を得ることができ
た。SUMMARY OF THE INVENTION The present invention focuses on the fact that many radionuclides emit a plurality of gamma rays, and measures them by a multiple gamma ray detector comprising a plurality of gamma ray detectors. By analyzing the obtained two-dimensional matrix, a method for qualitatively and quantitatively determining these nuclides was devised. According to this method, an energy resolution 1000 times higher than that of a conventional one-dimensional spectrum could be obtained.
【００１４】本発明の２次元マトリクス法は、試料中の
放射性核種から同時に発生した複数のガンマ線を多重ガ
ンマ線検出装置の２台以上の検出器で検出し、得られた
２個のガンマ線エネルギーを縦軸と横軸とする２次元マ
トリクス上に加算し、そのピークを検出する方法であ
り、１次元スペクトルのバックグラウンドが２次元平面
上で局在するために、ほとんどの領域で数カウント以下
に押さえられるため、微弱なピークの検出が可能にな
り、検出感度が上がる。In the two-dimensional matrix method of the present invention, a plurality of gamma rays simultaneously generated from radionuclides in a sample are detected by two or more detectors of a multiple gamma ray detector, and the obtained two gamma ray energies are longitudinally detected. This method detects peaks by adding them on a two-dimensional matrix with the axis and the horizontal axis. Since the background of the one-dimensional spectrum is localized on a two-dimensional plane, it is suppressed to a few counts or less in most regions. Therefore, a weak peak can be detected, and the detection sensitivity increases.
【００１５】また、本発明では、化学分離などの人為的
操作を必要としないため、計算機によるオンライン化が
可能である。つまり予め検出器のエネルギーと検出効率
の校正を行っておけば、試料を測定しながら２次元マト
リクスを生成し、その位置から核種の種類を特定し、同
時に計算機に内蔵した核種毎の核データを参照して、マ
トリクス上のピークの強度から核種の定量を行い、実時
間で結果を表示することが可能になる。当然ながら、半
減期の長い核種の定量も高速化される。Further, according to the present invention, since an artificial operation such as chemical separation is not required, online operation by a computer is possible. In other words, if the energy and detection efficiency of the detector are calibrated in advance, a two-dimensional matrix is generated while measuring the sample, the type of nuclide is specified from the position, and simultaneously the nuclide data for each nuclide built into the computer is obtained. As a reference, it is possible to determine the nuclide from the intensity of the peak on the matrix and display the result in real time. Naturally, the quantification of long-lived nuclides is also accelerated.
【００１６】同様にして、本発明においては、中性子放
射化法により放射化された試料中の核種の定性及び定量
分析も可能になる。Similarly, in the present invention, qualitative and quantitative analysis of nuclides in a sample activated by the neutron activation method becomes possible.
【００１７】[0017]
【発明の実施の形態】（１）中性子放射化法により放射
化された試料中の核種の定性及び定量分析 複数のゲルマニウム半導体検出器からなる多重ガンマ線
検出器を用いて放射化させた試料から発せられる複数の
ガンマ線を測定し、同時に観測された２本のガンマ線の
組み合わせをコンピューターに記録し、これを解析する
事により２次元スペクトルを作った。ここから任意のエ
ネルギーを有するガンマ線と同時に観測されたガンマ線
のスペクトルを作ると他の核種からのガンマ線にほとん
ど妨害されないきれいなスペクトルを得る事が出来る。
これにより化学分離などの操作を行わなくても共存する
核種からのガンマ線に妨害される事無く微量成分からの
ガンマ線を測定する事ができる。DESCRIPTION OF THE PREFERRED EMBODIMENTS (1) Qualitative and quantitative analysis of nuclides in a sample activated by a neutron activation method Emission from a sample activated using a multiple gamma ray detector comprising a plurality of germanium semiconductor detectors. A plurality of gamma rays obtained were measured, a combination of two gamma rays observed at the same time was recorded in a computer, and a two-dimensional spectrum was created by analyzing the combination. From this, if a gamma ray spectrum having an arbitrary energy is observed and a gamma ray spectrum observed at the same time is created, a clean spectrum hardly obstructed by gamma rays from other nuclides can be obtained.
Thus, gamma rays from trace components can be measured without being hindered by gamma rays from coexisting nuclides without performing operations such as chemical separation.
【００１８】本発明の検出方法においては、図２に示さ
れるように、原子炉からの熱中性子照射による放射化試
料１から同時に発生するガンマ線を多重ガンマ線検出装
置４で同時に計数測定し、垂直軸をカウント（強さ）、
縦軸及び横軸をガンマ線エネルギーとした２次元マトリ
ックス５を作成する。この方法では、試料中の放射性核
種から同時に発生する２本のガンマ線γ1、γ2を多重ガ
ンマ線検出装置で同時測定して、１次元スペクトルの代
りに２次元マトリックスを作成する。そのために、多核
種を含む試料においても化学分離等の処理なしに、１０
００倍のガンマ線分解能が達成され、核種の完全分離測
定が可能となった。図２にでは、縦軸及び横軸はそれぞ
れガンマ線エネルギーを表すので、その縦軸にγ1の値
が入り、その横軸にγ2の値が入ることによって定まっ
た位置で核種の種類が特定でき、また、その位置に示さ
れるピークの高さを垂直軸（カウント）により測定して
その核種の存在量が検出される。In the detection method of the present invention, as shown in FIG. 2, gamma rays simultaneously generated from an activated sample 1 by irradiation with thermal neutrons from a nuclear reactor are simultaneously counted and measured by a multiple gamma ray detector 4, and the vertical axis is measured. Count (strength),
A two-dimensional matrix 5 in which the vertical and horizontal axes are gamma ray energy is created. In this method, two gamma rays γ 1 and γ 2 simultaneously generated from radionuclides in a sample are simultaneously measured by a multiple gamma ray detector to create a two-dimensional matrix instead of a one-dimensional spectrum. Therefore, even for a sample containing multinuclides, without treatment such as chemical separation.
A gamma ray resolution of 00 times was achieved, and a complete separation measurement of nuclides became possible. In Figure 2, since the vertical and horizontal axes respectively represent the gamma ray energy, its longitudinal axis contains a value of gamma 1, certain types of nuclides in a position definite by the value of the gamma 2 in the horizontal axis fall The nuclide abundance can be detected by measuring the height of the peak indicated at that position on the vertical axis (count).
【００１９】又、図３に示されるように、放射化された
152Ｅｕからは８４１．６ｋｅＶ及び１２１．８ｋｅＶ
の２本のガンマ線が同時に発生する。この２本のガンマ
線を多重ガンマ線検出装置で同時に計数測定を行って２
次元マトリックスを作成した。Further, as shown in FIG.
841.6 keV and 121.8 keV from 152 Eu
Are simultaneously generated. The two gamma rays are simultaneously counted and measured by a multiplex gamma ray detector to obtain 2 gamma rays.
A dimensional matrix was created.
【００２０】図３は、図２のように、縦軸及び横軸がそ
れぞれガンマ線エネルギーを表したもので、その中で特
に縦軸を１００から１４０ｋｅＶ、横軸を８２０から８
６０ｋｅＶの範囲に拡大している。FIG. 3 shows, as in FIG. 2, the ordinate and the abscissa respectively represent the gamma ray energies. In particular, the ordinate represents 100 to 140 keV and the abscissa represents the 820 to 8
The range has been expanded to 60 keV.
【００２１】図３の下方の拡大図からは、152Ｅｕから
発生する２本のガンマ線１２１．８ｋｅＶと８４１．６
ｋｅＶが同時に記録され、この位置によって核種の種類
が特定できた。このようにして、４９元素の最高ｐｐｂ
（１０-9）オーダーの同時定量が可能になった。From the enlarged view at the bottom of FIG. 3, two gamma rays generated from 152 Eu, 121.8 keV and 841.6, are obtained.
keV was recorded at the same time, and the type of nuclide could be identified by this position. Thus, the highest ppb of 49 elements
Simultaneous quantification of (10 -9 ) orders is now possible.
【００２２】本発明においては、多重ガンマ線検出装置
は高い検出効率を有するため試料はミリグラムオーダー
で足りる。また、非破壊検査のため放射化試料をそのま
ま測定できるため非常に簡便であり、広範囲の試料にも
適応できる。例えば、環境試料や生体試料における微量
な金属元素の定量や地球科学あるいは隕石の分析など宇
宙科学の分野での利用が期待できる。In the present invention, since the multiple gamma ray detector has a high detection efficiency, a sample on the order of milligrams is sufficient. Further, since the activated sample can be measured as it is for nondestructive inspection, it is very simple and can be applied to a wide range of samples. For example, it can be expected to be used in the field of space science, such as quantification of trace metal elements in environmental samples and biological samples, and earth science or meteorite analysis.
【００２３】更にまた、129I（半減期1570万年）や 244
Pu（ 8080万年）を用いた年代測定が提案されている
が、これらの核種を本方法で分析することにより、年代
測定への応用も期待できる。さらに近年、生体内での微
量元素濃度と生体機能との関連が明らかになりつつある
が、本方法では広範囲の元素を同時に測定できるため、
今まで見逃されてきた微量元素の量を調べて、その効果
を新たに研究することが可能になる。Further, 129 I (half life of 15.7 million years) and 244
Although dating using Pu (80.8 million years) has been proposed, analysis of these nuclides by this method can be expected to be applied to dating. Furthermore, in recent years, the relationship between the trace element concentration in the living body and the biological function has been clarified, but this method can simultaneously measure a wide range of elements,
By examining the amount of trace elements that have been overlooked so far, it is possible to study their effects anew.
【００２４】（２）放射性試料中の核種の定性及び定量
分析 複数のガンマ線検出器からなる多重ガンマ線検出装置を
用いて放射性試料から発せられる複数の同時発生ガンマ
線を測定し、そのガンマ線対のエネルギー情報を事象毎
にコンピューターに記録し、これを解析して２次元マト
リクスを作った。これをマトリクス上にて、あるいは一
方の軸に狭いゲートを設定して、１次元スペクトルを切
り取った上で、実効的に２次元ピークの強度を測定す
る。ガンマ線のエネルギーと強度について事前に校正を
行っておくことにより、２次元ピークのチャンネルとピ
ーク面積は、エネルギーと強度に変換される。これらを
基に、核種の定量が可能になる。(2) Qualitative and quantitative analysis of nuclides in a radioactive sample A plurality of simultaneous gamma rays emitted from a radioactive sample are measured using a multiple gamma ray detector comprising a plurality of gamma ray detectors, and energy information of the gamma ray pair is measured. Was recorded on a computer for each event and analyzed to create a two-dimensional matrix. This is set on a matrix or a narrow gate is set on one axis to cut out a one-dimensional spectrum, and then effectively measure the intensity of a two-dimensional peak. By calibrating the energy and intensity of gamma rays in advance, the channel and peak area of the two-dimensional peak are converted into energy and intensity. Based on these, quantification of nuclides becomes possible.
【００２５】以上の操作は事前に標準線源を測定して検
出器の校正を行っておくことにより、オンラインで解析
することが可能になる。そのために、予めエネルギーと
その強度の判っている標準線源を測定して、検出器毎に
エネルギーと検出効率の校正データを作成する。試料を
測定しながら検出器のエネルギーを校正して２次元マト
リクスを生成する。同時に計算機に内蔵した核種毎の核
データを参照して、マトリクス上のピークの強度から検
出効率の校正データを基に核種の定量を行い、実時間で
結果を表示することが可能になる。当然ながら、半減期
の長い長寿命核種の定量も、短寿命核種がなくなるのを
待つ必要はなく、分析が高速化される。The above operation can be analyzed on-line by measuring the standard radiation source and calibrating the detector in advance. For this purpose, a standard source whose energy and intensity are known in advance is measured, and calibration data of energy and detection efficiency is created for each detector. While measuring the sample, the energy of the detector is calibrated to generate a two-dimensional matrix. At the same time, by referring to the nuclear data for each nuclide incorporated in the computer, the nuclide can be quantified based on the calibration data of the detection efficiency from the peak intensity on the matrix, and the result can be displayed in real time. Naturally, the quantification of long-lived nuclides with a long half-life does not have to wait for the short-lived nuclides to run out, and the analysis is speeded up.
【００２６】以上の発明で使用する多重ガンマ線検出装
置は、最低２台以上のガンマ線検出器から構成する。２
台の検出器からの信号を速い同時計数回路にて、同時計
数事象のみを選別する。その時に、２つの検出器からの
エネルギー情報を計算機に取り込む。この情報を基にし
て、２つのガンマ線の相関を２次元マトリクス上に事象
の頻度分布を作る。必ずしも、２次元マトリクスでなく
とも、それに代わるものであれば良い。また、多重ガン
マ線検出装置の性能は、検出器の台数が多いほど、また
個々の検出器の検出効率が高ければ高い程良い。さらに
ＢＧＯサプレッサーなどと組み合わせると、バックグラ
ウンドを押さえて感度が良くすることができる。The multiplex gamma ray detector used in the above invention comprises at least two or more gamma ray detectors. 2
The signals from the two detectors are sorted by a fast coincidence circuit only for coincidence events. At that time, energy information from the two detectors is taken into the computer. Based on this information, a correlation between two gamma rays is used to create a frequency distribution of events on a two-dimensional matrix. It is not always necessary to use a two-dimensional matrix as long as it is a substitute for the matrix. Further, the performance of the multiple gamma ray detecting device is better as the number of detectors is larger and the detection efficiency of each detector is higher. Further, when combined with a BGO suppressor or the like, the sensitivity can be improved by suppressing the background.
【００２７】[0027]
【実施例】（実施例１）中性子放射化法と組み合わせた
微量元素定量法 標準岩石試料を原子炉で中性子照射を行い放射化した試
料からのガンマ線を多重ガンマ線検出装置で測定した。
約１００ミリグラムの試料を１０分間原子炉で放射化し
て発せられるガンマ線を約４日間多重ガンマ線測定装置
で測定した。EXAMPLES Example 1 Trace Element Determination Method Combined with Neutron Activation Method A standard rock sample was irradiated with neutrons in a nuclear reactor, and gamma rays from the activated sample were measured with a multiple gamma ray detector.
Approximately 100 milligrams of the sample were activated in a nuclear reactor for 10 minutes, and the gamma rays emitted were measured for about 4 days with a multiple gamma ray measuring device.
【００２８】即ち、通産省工業技術院地質調査所の発行
している標準岩石試料ＪＢ−１及びＪＰ−１を原研研究
炉ＪＲＲ−４で中性子照射を行い、原研東海研究所タン
デム加速器施紋の多重ガンマ線検出装置”ＧＥＭＩＮ
Ｉ”で１−４日間測定を行った。That is, the standard rock samples JB-1 and JP-1 issued by the Geological Survey of the Ministry of International Trade and Industry of Japan were irradiated with neutrons by the JAERI research reactor JRR-4, and the tandem accelerators of JAERI were multiplexed. Gamma ray detector "GEMIN"
The measurement was carried out at I ″ for 1-4 days.
【００２９】ここでは、化学分離等の人為的な操作を行
わず、また短寿命の核種の崩壊を待つ必要もなく、照射
後即測定を開始し、短時間で、２７核種の元素が同時に
定量できた。測定された元素は、ガンマ線の強度からそ
の含有量を計算すると、これまでに得られている文献値
と誤差の範囲内で一致した。 また、同じ手法で４９元
素の同時定量が可能であることを明らかにした。２次元
マトリクスではバックグラウンドが大幅に低減するた
め、微弱なピークの検出が可能になり、存在比１０
-9（１０億分の１）オーダーの核種の定量ができるよう
になった。Here, the measurement is started immediately after irradiation without performing any artificial operation such as chemical separation, and without having to wait for the decay of short-lived nuclides, and the elements of 27 nuclides are simultaneously quantified in a short time. did it. When the content of the measured element was calculated from the intensity of the gamma ray, it coincided with the literature values obtained so far within an error range. In addition, it was clarified that simultaneous quantification of 49 elements was possible by the same method. In the two-dimensional matrix, the background is greatly reduced, so that a weak peak can be detected.
It has become possible to quantify nuclides on the order of -9 (one billionth).
【００３０】本発明で使用された多重ガンマ線検出装
置”ＧＥＭＩＮＩ”とは、ＢＧＯコンプトンサプレッサ
ーとゲルマニウム検出器を組み合わせたアンチコンプト
ンガンマ線分析器が、低バックグラウンド・高分解能を
達成できるので、これを多数組み合わせて球状に配置し
た装置である。様々な核反応により作られた原子核の高
励起状態からのガンマ線を測定して、それらの内部構造
を調べるのを主目的として平成１０年７月に完成した。
原研東海研タンデム加速器施設での重イオンビームを用
いた核分光実験で多くの実績を納めている。The multi-gamma ray detector "GEMINI" used in the present invention is an anti-Compton gamma ray analyzer which combines a BGO Compton suppressor and a germanium detector, and can achieve low background and high resolution. It is a device that is arranged in a spherical shape in combination. It was completed in July 1998 mainly for measuring gamma rays from highly excited states of nuclei generated by various nuclear reactions and examining their internal structures.
He has achieved many achievements in nuclear spectroscopy experiments using heavy ion beams at the JAERI Tokai tandem accelerator facility.
【００３１】本実施例において、新しい検出法で同時定
量可能となった元素（４９種類）は、Ａｇ，Ａｓ，Ｂ
ａ，Ｂｒ，Ｃａ，Ｃｄ，Ｃｅ，Ｃｌ，Ｃｏ，Ｃｓ，Ｅ
ｒ，Ｅｕ，Ｆｅ，Ｇａ，Ｇｄ，Ｇｅ，Ｈｆ，Ｈｇ，Ｉ，
Ｉｎ，Ｉｒ，Ｋ，Ｌａ，Ｌｕ，Ｍｎ，Ｍｏ，Ｎａ，Ｎ
ｄ，Ｎｅ，Ｎｉ，Ｏｓ，Ｐｔ，Ｒａ，Ｒｂ，Ｒｅ，Ｒ
ｕ，Ｓｂ，Ｓｃ，Ｓｅ，Ｓｍ，Ｓｎ，Ｔａ，Ｔｂ，Ｔ
ｈ，Ｔｉ，Ｕ，Ｗ，Ｙｂ，Ｚｎであり、その検出限界は
１０-2−１０-3（重量比）である。In this embodiment, the elements (49 types) that can be simultaneously quantified by the new detection method are Ag, As, B
a, Br, Ca, Cd, Ce, Cl, Co, Cs, E
r, Eu, Fe, Ga, Gd, Ge, Hf, Hg, I,
In, Ir, K, La, Lu, Mn, Mo, Na, N
d, Ne, Ni, Os, Pt, Ra, Rb, Re, R
u, Sb, Sc, Se, Sm, Sn, Ta, Tb, T
h, Ti, U, W, Yb, and Zn, and their detection limits are 10 −2 −10 −3 (weight ratio).
【００３２】これに対し、従来の放射化分析法（一次元
スペクトル）で可能な元素は次の２３種である。Ａｌ，
Ａｒ，Ａｕ，Ｃｒ，Ｃｕ，Ｄｙ，Ｆ，Ｈｏ，Ｋｒ，Ｍ
ｇ，Ｎｂ，Ｐｄ，Ｐｒ，Ｒｈ，Ｓ，Ｓｒ，Ｔｅ，Ｔｌ，
Ｔｍ，Ｖ，Ｘｅ，Ｙ，Ｚｒその検出限界は１０-2−１０
-3（重量比）である。On the other hand, the following 23 kinds of elements are available by the conventional activation analysis (one-dimensional spectrum). Al,
Ar, Au, Cr, Cu, Dy, F, Ho, Kr, M
g, Nb, Pd, Pr, Rh, S, Sr, Te, Tl,
Tm, V, Xe, Y, Zr The detection limit is 10 -2 -10
-3 (weight ratio).
【００３３】（実施例２）アクチノイド元素の分析 マイナーアクチノイド核種の核変換基礎データを計るこ
とは、原子力研究にとって重要な基礎研究である。この
ためにマイナーアクチノイドの定量が必要であるが、こ
れまでは主にアルファ線の測定によるところが大きかっ
た。しかしながら、近傍の核種は似たエネルギーのアル
ファ線を放出するので高分解能で検出する必要がある
が、アルファ線は物質中でのエネルギーロスが大きいの
で、試料の化学分離を行い、不純物を除いた上で、乾固
して薄い線源にする必要があった。これには特殊な技能
が必要であるばかりでなく、時として高い分離効率を得
ることは難しかった。(Example 2) Analysis of actinoid elements Measuring basic transmutation data of minor actinoid nuclides is an important basic research for nuclear power research. For this purpose, the quantification of minor actinoids is necessary, but until now mainly the measurement by alpha rays has been large. However, nuclides in the vicinity emit alpha rays of similar energy and need to be detected with high resolution.Although alpha rays have a large energy loss in the substance, chemical separation of the sample was performed to remove impurities. Above, it was necessary to dry to a thin source. This not only required special skills, but sometimes it was difficult to obtain high separation efficiency.
【００３４】多重ガンマ線検出法においては、多重ガン
マ線を発生するという条件はあるものの、これらの問題
点は解決され、化学分離なしに高精度の分析が可能にな
った。事実ＧＥＭＩＮＩを用いた２３７Ｎｐ標準線源の
測定において０．０１べクレルの強度まで、完全に他の
核種と分離して測定することができた。In the multiple gamma ray detection method, although there is a condition that multiple gamma rays are generated, these problems have been solved and high-precision analysis without chemical separation has become possible. In fact, in the measurement of a 237 Np standard source using GEMINI, it was possible to completely separate from other nuclides up to an intensity of 0.01 becquerel.
【００３５】[0035]
【発明の効果】本発明により、一般に地質学的試料の中
性子照射では、24Ｎａ及び56Ｍｎからの強いガンマ線が
観測されるため微量成分からのガンマ線を測定する事は
困難であるが、多重ガンマ線分析法により化学分離を行
う事無く同時に２７元素からのガンマ線を観測する事が
できた。また測定された元素はガンマ線の強度からその
含有量を計算すると誤差の範囲内で標準岩石試料の文献
値と一致していた。According to the present invention, it is generally difficult to measure gamma rays from trace components by neutron irradiation of geological samples because strong gamma rays from 24 Na and 56 Mn are observed. Gamma rays from 27 elements could be observed at the same time without chemical separation by the analytical method. When the content of the measured elements was calculated from the intensity of gamma rays, they were consistent with the literature values of the standard rock samples within the range of error.
【００３６】このことから本発明が定性分析だけでなく
定量分析にも適応できる事がわかる。検出された元素の
中でＥｕは僅か４ｐｐｂの含有量であるが、これも化学
分離をする事無く他の元素と同時に測定する事ができ
た。 さらに条件が整えば４９元素にこの方法を適用す
る事ができる。This shows that the present invention can be applied not only to qualitative analysis but also to quantitative analysis. Among the detected elements, Eu has a content of only 4 ppb, but this could be measured simultaneously with other elements without chemical separation. If conditions are further satisfied, this method can be applied to 49 elements.
【００３７】又、本発明により、一般に多数の放射性核
種が存在する場合には、その各々を完全に分離して定量
する事は不可能であるが、多重ガンマ線検出法では従来
よりも分解能が格段に改善され、いかに多くの核種を含
む場合でも、化学分離等の副次的手段を用いることな
く、完全分離・完全定量を可能にした。In addition, according to the present invention, when a large number of radionuclides are present, it is generally impossible to completely separate and quantify each of them. However, the multiple gamma ray detection method has a much higher resolution than before. This enables complete separation and complete quantification without using secondary means such as chemical separation, no matter how many nuclides are included.
【図１】 従来の放射化試料の検出方法を示す図であ
る。FIG. 1 is a diagram showing a conventional method for detecting an activated sample.
【図２】 本発明の放射化試料の検出方法を示す図であ
る。FIG. 2 is a diagram showing a method for detecting an activated sample of the present invention.
【図３】 本発明の検出法で作成した２次元マトリック
スを示す図である。FIG. 3 is a diagram showing a two-dimensional matrix created by the detection method of the present invention.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 早川 岳人 茨城県那珂郡東海村白方字白根２番地の４ 日本原子力研究所東海研究所内 (72)発明者 藤 暢輔 茨城県那珂郡東海村白方字白根２番地の４ 日本原子力研究所東海研究所内 (72)発明者 篠原 伸夫 茨城県那珂郡東海村白方字白根２番地の４ 日本原子力研究所東海研究所内 Ｆターム(参考） 2G001 AA04 BA01 CA02 DA02 GA01 JA11 KA01 KA14 LA01 LA03 NA07 NA10 NA11 NA12 NA13 NA17 2G088 EE25 EE30 FF04 FF15 GG21 KK01 KK15 KK24 KK29 LL02 LL06 LL11 ──────────────────────────────────────────────────続 き Continuing on the front page (72) Inventor Taketo Hayakawa 2-4 Shirane, Shirakata, Tokai-mura, Naka-gun, Ibaraki Pref. Japan Atomic Energy Research Institute Tokai Research Institute (72) Inventor Nobusuke Fuji Tokai-mura, Naka-gun, Ibaraki No. 2 at Shirane in the Japan Atomic Energy Research Institute, Tokai Research Laboratory (72) Nobuo Shinohara, Inventor Nobuo Shinohara, No. 2 at Shirane, Shikata in Tokai Village, Naka-gun, Ibaraki Prefecture CA02 DA02 GA01 JA11 KA01 KA14 LA01 LA03 NA07 NA10 NA11 NA12 NA13 NA17 2G088 EE25 EE30 FF04 FF15 GG21 KK01 KK15 KK24 KK29 LL02 LL06 LL11
Claims (3)
合わせることより、中性子その他の粒子線或いはガンマ
線により放射化された試料中の核種から発生するガンマ
線対（ペア）を多重ガンマ線検出装置により測定して試
料中の核種を分析する方法。1. A gamma ray pair generated from a neutron or other nuclide in a sample activated by a particle beam or gamma ray by a multiplex gamma ray detector by combining the multiplex gamma ray detection method and the activation analysis method. A method of measuring and analyzing nuclides in a sample.
するガンマ線対を多重ガンマ線検出装置で同時に測定し
て２次元マトリックスを作成することにより、試料中の
核種を分離することなく各核種を分離して測定すること
を特徴とする請求項１記載の方法。2. A two-dimensional matrix is created by simultaneously measuring gamma ray pairs simultaneously generated from activated nuclides in a sample with a multiple gamma ray detector, thereby separating each nuclide without separating the nuclides in the sample. The method according to claim 1, wherein the measurement is performed separately.
マ線検出装置を用いて試料中に存在する多数の放射性核
種から発せられる複数の同時発生ガンマ線を測定し、各
核種からのガンマ線対のエネルギー情報をコンピュータ
ーに記録し、これを解析して縦軸及び横軸をガンマ線エ
ネルギーとした２次元マトリクスを作成し、このマトリ
クス上に形成された位置から各核種を特定し、その各ピ
ークを予めエネルギーとその強度の判っている標準線源
と比較して試料中の核種の含有量を測定することによ
り、各核種の定性、定量分析を行うことを特徴とする多
重ガンマ線検出により放射性核種を分析する方法。3. A multi-gamma ray detector comprising a plurality of gamma ray detectors is used to measure a plurality of simultaneous gamma rays emitted from a large number of radionuclides present in a sample, and energy information of a gamma ray pair from each nuclide is measured. It is recorded on a computer and analyzed to create a two-dimensional matrix with gamma-ray energies on the vertical and horizontal axes, identify each nuclide from the positions formed on this matrix, and determine the peaks and the energy and A method for analyzing radionuclide by multiple gamma ray detection, characterized in that qualitative and quantitative analysis of each nuclide is performed by measuring the content of nuclide in a sample in comparison with a standard radiation source whose intensity is known.
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| JP2010101663A (en) * | 2008-10-22 | 2010-05-06 | Japan Atomic Energy Agency | Multiple radiation analyzing apparatus and multiple radiation analyzing method |
| JP2013036774A (en) * | 2011-08-04 | 2013-02-21 | Hitachi Ltd | Radiation detection apparatus and detection method |
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| CN110990783A (en) * | 2019-11-14 | 2020-04-10 | 中国核电工程有限公司 | Method for calculating relative content of Pu-242 nuclide |
| CN113466323A (en) * | 2021-06-30 | 2021-10-01 | 应急管理部沈阳消防研究所 | Mass spectrum detection device and method for automatically evaluating protective performance of mask |
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| JPH01210892A (en) * | 1988-02-19 | 1989-08-24 | Nogyo Doboku Shikenjo | Method for tracing water flow |
| JPH11194170A (en) * | 1998-01-06 | 1999-07-21 | Hitachi Ltd | Radioactive material inspection device and radioactive waste inspection system |
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Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH01210892A (en) * | 1988-02-19 | 1989-08-24 | Nogyo Doboku Shikenjo | Method for tracing water flow |
| JPH11194170A (en) * | 1998-01-06 | 1999-07-21 | Hitachi Ltd | Radioactive material inspection device and radioactive waste inspection system |
Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2005114387A (en) * | 2003-10-03 | 2005-04-28 | Japan Atom Energy Res Inst | Method of analyzing nuclide highly sensitively by concurrent counting measurement with one radiation detector |
| JP2010101663A (en) * | 2008-10-22 | 2010-05-06 | Japan Atomic Energy Agency | Multiple radiation analyzing apparatus and multiple radiation analyzing method |
| JP2013036774A (en) * | 2011-08-04 | 2013-02-21 | Hitachi Ltd | Radiation detection apparatus and detection method |
| RU2698468C1 (en) * | 2018-06-18 | 2019-08-27 | Объединенный Институт Ядерных Исследований (Оияи) | Method of simulating chemical behavior of atoms of superheavy elements |
| CN110501740A (en) * | 2019-08-23 | 2019-11-26 | 南京核安核能科技有限公司 | A kind of anti-antiuniverse X-ray spectrometer X HPGe detector detection method of health of background digitlization |
| CN110990783A (en) * | 2019-11-14 | 2020-04-10 | 中国核电工程有限公司 | Method for calculating relative content of Pu-242 nuclide |
| CN110990783B (en) * | 2019-11-14 | 2024-03-19 | 中国核电工程有限公司 | Calculation method of Pu-242 nuclide relative content |
| CN113466323A (en) * | 2021-06-30 | 2021-10-01 | 应急管理部沈阳消防研究所 | Mass spectrum detection device and method for automatically evaluating protective performance of mask |
| CN113466323B (en) * | 2021-06-30 | 2024-04-26 | 应急管理部沈阳消防研究所 | Mass spectrum detection device and method for automatically evaluating mask protective performance |
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